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Using femtosecond time-resolved X-ray diffraction, we investigated optically excited coherent acoustic phonons in the Weyl semimetal TaAs. The low symmetry of the (112) surface probed in our experiment enables the simultaneous excitation of longitudinal and shear acoustic modes, whose dispersion closely matches our simulations. We observed an asymmetry in the spectral lineshape of the longitudinal mode that is notably absent from the shear mode, suggesting a time-dependent frequency chirp that is likely driven by photoinduced carrier diffusion. We argue on the basis of symmetry that these acoustic deformations can transiently alter the electronic structure near the Weyl points and support this with model calculations. Our study underscores the benefit of using off-axis crystal orientations when optically exciting acoustic deformations in topological semimetals, allowing one to transiently change their crystal and electronic structures., Comment: 6 pages, 4 figures for manuscript, and 15 pages and 11 figures for supplemental materials

The discovery of two-dimensional (2D) systems hosting intrinsic long-range magnetic order represents a seminal addition to the rich physical landscape of van der Waals (vdW) materials. CrI3 has emerged as perhaps the most salient example, as the interdependence of crystalline structure and magnetic order, along with strong light-matter interactions provides a promising platform to explore the optical control of magnetic, vibrational, and charge degrees of freedom at the 2D limit. However, the fundamental question of how this relationship between structure and magnetism manifests on their intrinsic timescales has rarely been explored. Here, we use ultrafast optical spectroscopy to probe magnetic and vibrational dynamics in CrI3, revealing demagnetization dynamics governed by spin-flip scattering and remarkably, a strong transient exchange-mediated interaction between lattice vibrations and spin oscillations. The latter yields a coherent spin-coupled phonon mode that is highly sensitive to the helicity of the driving pulse in the magnetically ordered phase. Our results shed light on the nature of spin-lattice coupling in vdW magnets on ultrafast timescales and highlight their potential for applications requiring non-thermal, high-speed control of magnetism at the nanoscale., Comment: 7 pages, 3 figures

Ultrafast pump-probe technique is a powerful tool to understand and manipulate properties of materials for designing novel quantum devices. An intense, single cycle terahertz pulse can change the intrinsic properties of semiconductor quantum dots to have different luminescence. In a hybrid system of plasmon and exciton, the coherence and coupling between these two degrees of freedom play an important role on their optical properties. Therefore, we consider a terahertz pump optical probe experiment in the hybrid systems where the terahertz pump pulse couples to the exciton degrees of freedom on the quantum dot. The time resolved photoluminescence of the hybrid system shows that the response of the characteristic frequency shifts according to the overlap between the pump and probe pulses. Furthermore, the resonance between the exciton and plasmons can be induced by the terahertz pump pulse in some parameter regimes. Our results show the terahertz driven hybrid system can be a versatile tool for manipulating the material properties and open a new route to design modern optical devices., Comment: 8 pages, 4 figures, and supplemental materials included

Symmetry plays a central role in conventional and topological phases of matter, making the ability to optically drive symmetry change a critical step in developing future technologies that rely on such control. Topological materials, like the newly discovered topological semimetals, are particularly sensitive to a breaking or restoring of time-reversal and crystalline symmetries, which affect both bulk and surface electronic states. While previous studies have focused on controlling symmetry via coupling to the crystal lattice, we demonstrate here an all-electronic mechanism based on photocurrent generation. Using second-harmonic generation spectroscopy as a sensitive probe of symmetry change, we observe an ultrafast breaking of time-reversal and spatial symmetries following femtosecond optical excitation in the prototypical type-I Weyl semimetal TaAs. Our results show that optically driven photocurrents can be tailored to explicitly break electronic symmetry in a generic fashion, opening up the possibility of driving phase transitions between symmetry-protected states on ultrafast time scales., Comment: 28 pages, 15 figures, 4 Tables

We investigate polarization-dependent ultrafast photocurrents in the Weyl semimetal TaAs using terahertz (THz) emission spectroscopy. Our results reveal that highly directional, transient photocurrents are generated along the non-centrosymmetric c-axis regardless of incident light polarization, while helicity-dependent photocurrents are excited within the ab-plane. This is consistent with earlier static photocurrent experiments, and demonstrates on the basis of both the physical constraints imposed by symmetry and the temporal dynamics intrinsic to current generation and decay that optically induced photocurrents in TaAs are inherent to the underlying crystal symmetry of the transition metal monopnictide family of Weyl semimetals.

Intense, single-cycle terahertz (THz) pulses offer a promising approach for understanding and controlling the properties of a material on an ultrafast time scale. In particular, resonantly exciting phonons leads to a better understanding of how they couple to other degrees of freedom in the material (e.g., ferroelectricity, conductivity and magnetism) while enabling coherent control of lattice vibrations and the symmetry changes associated with them. However, an ultrafast method for observing the resulting structural changes at the atomic scale is essential for studying phonon dynamics. A simple approach for doing this is optical second harmonic generation (SHG), a technique with remarkable sensitivity to crystalline symmetry in the bulk of a material as well as at surfaces and interfaces. This makes SHG an ideal method for probing phonon dynamics in topological insulators (TI), materials with unique surface transport properties. Here, we resonantly excite a polar phonon mode in the canonical TI Bi$_2$Se$_3$ with intense THz pulses and probe the subsequent response with SHG. This enables us to separate the photoinduced lattice dynamics at the surface from transient inversion symmetry breaking in the bulk. Furthermore, we coherently control the phonon oscillations by varying the time delay between a pair of driving THz pulses. Our work thus demonstrates a versatile, table-top tool for probing and controlling ultrafast phonon dynamics in materials, particularly at surfaces and interfaces, such as that between a TI and a magnetic material, where exotic new states of matter are predicted to exist.

We have studied the sub-picosecond quasiparticle dynamics in the perovskite manganite La0.7Ca0.3MnO3 and the layered manganite La1.4Sr1.6Mn2O7 using ultrafast optical spectroscopy. We found that for T > TC, initial relaxation proceeds on the time scale of several hundred femtoseconds and corresponds to the redressing of a photoexcited electron to its polaronic ground state. The temperature and dimensionality dependence of this polaron redressing time provides insight into the relationship between polaronic motion and spin dynamics on a sub-picosecond time scale. We also observe a crossover to a more conventional electron-phonon relaxation in the ferromagnetic metallic phase below Tc.

Strong coupling between discrete phonon and continuous electron-hole pair excitations can give rise to a pronounced asymmetry in the phonon line shape, known as the Fano resonance. This effect has been observed in a variety of systems, such as stripe-phase nickelates, graphene and high-$T_{c}$ superconductors. Here, we reveal explicit evidence for strong coupling between an infrared-active $A_1$ phonon and electronic transitions near the Weyl points (Weyl fermions) through the observation of a Fano resonance in the recently discovered Weyl semimetal TaAs. The resultant asymmetry in the phonon line shape, conspicuous at low temperatures, diminishes continuously as the temperature increases. This anomalous behavior originates from the suppression of the electronic transitions near the Weyl points due to the decreasing occupation of electronic states below the Fermi level ($E_{F}$) with increasing temperature, as well as Pauli blocking caused by thermally excited electrons above $E_{F}$. Our findings not only elucidate the underlying mechanism governing the tunable Fano resonance, but also open a new route for exploring exotic physical phenomena through the properties of phonons in Weyl semimetals., Comment: 16 pages, 3 figures

We investigate spin dynamics in the antiferromagnetic (AFM) multiferroic TbMnO3 using optical- pump, terahertz (THz)-probe spectroscopy. Photoexcitation results in a broadband THz transmission change, with an onset time of 25 ps at 6 K that becomes faster at higher temperatures. We attribute this time constant to spin-lattice thermalization. The excellent agreement between our measurements and previous ultrafast resonant x-ray diffraction measurements on the same material confirms that our THz pulse directly probes spin order. We suggest that this could be the case in general for insulating AFM materials, if the origin of the static absorption in the THz spectral range is magnetic.

We report electric polarization and magnetization measurements in single crystals of double perovskite Lu2MnCoO6 using pulsed magnetic fields and optical second harmonic generation (SHG) in DC magnetic fields. we observe well-resolved magnetic field-induced changes in the electric polarization in single crystals and thereby resolve the question about whether multiferroic behavior is intrinsic to these materials or an extrinsic feature of polycrystals. We find electric polarization along the crystalline b-axis, that is suppressed by applying a magnetic fields along c-axis and advance a model for the origin of magnetoelectric coupling. We furthermore map the phase diagram using both capacitance and electric polarization to identify regions of ordering and regions of magnetoelectric hysteresis. This compound is a rare example of coupled hysteretic behavior in the magnetic and electric properties. The ferromagnetic-like magnetic hysteresis loop that couples to hysteretic polarization can be attributed not to ordinary ferromagnetic domains, but to the rich physics of magnetic frustration of Ising-like spins in the axial next-nearest neighbor interaction model., Comment: 5 pages, 5 figures

We demonstrate a new approach for directly measuring the ultrafast energy transfer between elec- trons and magnons, enabling us to track spin dynamics in an antiferromagnet (AFM). In multiferroic HoMnO3, optical photoexcitation creates hot electrons, after which changes in the spin order are probed with a THz pulse tuned to a magnon resonance. This reveals a photoinduced transparency, which builds up over several picoseconds as the spins heat up due to energy transfer from hot elec- trons via phonons. This spin-lattice thermalization time is ?10 times faster than that of typical ferromagnetic (FM) manganites. We qualitatively explain the fundamental differences in spin-lattice thermalization between FM and AFM systems and apply a Boltzmann equation model for treating AFMs. Our work gives new insight into spin-lattice thermalization in AFMs and demonstrates a new approach for directly monitoring the ultrafast dynamics of spin order in these systems.

We present a systematic study of both the temperature and frequency dependence of the optical response in TaAs, a material that has recently been realized to host the Weyl semimetal state. Our study reveals that the optical conductivity of TaAs features a narrow Drude response alongside a conspicuous linear dependence on frequency. The width of the Drude peak decreases upon cooling, following a $T^{2}$ temperature dependence which is expected for Weyl semimetals. Two linear components with distinct slopes dominate the 5-K optical conductivity. A comparison between our experimental results and theoretical calculations suggests that the linear conductivity below $\sim$230~cm$^{-1}$ is a clear signature of the Weyl points lying in very close proximity to the Fermi energy., Comment: 5 pages, 4 figures

We systematically measured the Hall effect in the extremely large magnetoresistance semimetal WTe$_2$. By carefully fitting the Hall resistivity to a two-band model, the temperature dependencies of the carrier density and mobility for both electron- and hole-type carriers were determined. We observed a sudden increase of the hole density below $\sim$160~K, which is likely associated with the temperature-induced Lifshitz transition reported by a previous photoemission study. In addition, a more pronounced reduction in electron density occurs below 50~K, giving rise to comparable electron and hole densities at low temperature. Our observations indicate a possible electronic structure change below 50~K, which might be the direct driving force of the electron-hole ``compensation'' and the extremely large magnetoresistance as well. Numerical simulations imply that this material is unlikely to be a perfectly compensated system., Comment: 10 pages, 3 figures. Supplemental material online

Ultrafast optical pump-probe spectroscopy is used to track carrier dynamics in the large magnetoresistance material WTe$_{2}$. Our experiments reveal a fast relaxation process occurring on a sub-picosecond time scale that is caused by electron-phonon thermalization, allowing us to extract the electron-phonon coupling constant. An additional slower relaxation process, occurring on a time scale of $\sim$5-15 picoseconds, is attributed to phonon-assisted electron-hole recombination. As the temperature decreases from 300 K, the timescale governing this process increases due to the reduction of the phonon population. However, below $\sim$50 K, an unusual decrease of the recombination time sets in, most likely due to a change in the electronic structure that has been linked to the large magnetoresistance observed in this material., Comment: 6 pages, 4 figures

We use optical pump--THz probe spectroscopy at low temperatures to study the hot carrier response in thin Bi$_2$Se$_3$ films of several thicknesses, allowing us to separate the bulk from the surface transient response. We find that for thinner films the photoexcitation changes the transport scattering rate and reduces the THz conductivity, which relaxes within 10 picoseconds (ps). For thicker films, the conductivity increases upon photoexcitation and scales with increasing both the film thickness and the optical fluence, with a decay time of approximately 5 ps as well as a much higher scattering rate. These different dynamics are attributed to the surface and bulk electrons, respectively, and demonstrate that long-lived mobile surface photo-carriers can be accessed independently below certain film thicknesses for possible optoelectronic applications., Comment: 4+ pages, 3 figures. Submitted

Ferroelectric and ferromagnetic materials possess spontaneous electric and magnetic order, respectively, which can be switched by the corresponding applied electric and magnetic fields. Multiferroics combine these properties in a single material, providing an avenue for controlling electric polarization with a magnetic field and magnetism with an electric field. These materials have been intensively studied in recent years, both for their fundamental scientific interest as well as their potential applications in a broad range of magnetoelectric devices [1, 2, 3, 4]. However, the microscopic origins of magnetism and ferroelectricity are quite different, and the mechanisms producing strong coupling between them are not always well understood. Hence, gaining a deeper understanding of magnetoelectric coupling in these materials is the key to their rational design. Here, we use ultrafast optical spectroscopy to show that quantum charge fluctuations can govern the interplay between electric polarization and magnetic ordering in the charge-ordered multiferroic LuFe2O4.